Industrial emissions are a notorious source of atmospheric pollution in the Cubatão industrial park of Southern Brazil, where dispersion is restricted by surrounding mountain ranges. It is shown here that road transport is also a large source of gases and aerosols, which can dominate pollutant concentrations at ground level, depending on meteorological conditions. SO2 was released mainly by industry, while road transport was a major source of NOx. Rapid removal of NO2 and SO2 was attributed to fast gas phase and heterogeneous reactions, respectively. Average PM10 concentrations increased by an order of magnitude during sea breeze fumigation, and high particulate pollution events were associated with vehicular activity. It is demonstrated that fast-response portable instrumentation can provide a useful alternative to measurements at fixed network sites for spatial (horizontal and vertical) mapping of atmospheric pollutants.